AU2012229849B2

AU2012229849B2 - Complex system for utilizing coal in manufacture of char and raw material gas and electric power generation

Info

Publication number: AU2012229849B2
Application number: AU2012229849A
Authority: AU
Inventors: Tatsuro Harada; Jun-Ichiro Hayashi; Seiichiro Matsuda; Yohsuke Matsushita; Isao Mochida; Toshiro Noguchi; Tsuyoshi Yamamoto
Original assignee: Kyushu Electric Power Co Inc; Kyushu University NUC
Current assignee: Kyushu Electric Power Co Inc; Kyushu University NUC
Priority date: 2011-03-15
Filing date: 2012-03-15
Publication date: 2016-08-04
Anticipated expiration: 2032-03-15
Also published as: US9334458B2; US20140030155A1; DE112012001242T5; JP5857340B2; JPWO2012124765A1; DE112012001242B4; WO2012124765A1; AU2012229849A1

Abstract

A large percentage of low-rank coal, which is abundant, has high moisture content and high oxygen content, and thus suffers from poor transportability. Further, when using such coal for heating, because of the loss of sensible heat of water and vaporization latent heat there is lowered thermal efficiency, and because of the high volatile matter content percentage, it is difficult to use such coal in existing coal combustion facilities. This combined system for manufacturing char/raw material gas from coal, and for generating electricity is provided with the following: a drying unit for drying low-rank coal that has high moisture content; a reformer for reforming the low-rank coal dried by the drying unit; a fluid bed furnace using the reformed coal obtained using the reformer as fuel; a producer gas supply pipe that supplies the combustion gas of the fluid bed furnace to the reformer as a thermal decomposition gasifier; and a catalyst reform device that reforms the producer gas and volatile components reformed by the reformer and obtained from the low-rank coal.

Description

DESCRIPTION

Title of Invention: COMPLEX SYSTEM FOR UTILIZING COAL IN MANUFACTURE OF CHAR AND RAW MATERIAL GAS AND ELECTRIC POWER GENERATION T e c h ni c a1 Field [0001] The present invention relates to a complex system which is capable of merging electric power generation and coal chemistry so as to utilize coal, the coal being highly utilized as heat, electricity, and a chemical raw material, for manufacture of char a n d r a w m a t e r i a 1 g a s a n d e 1 e c t r i c p o w e r g e n e r a t ion. T his i s a c h i e v e d by reforming dried low rank coal, while being moved in a moving bed reformer, and pyrolyzing and gasifying the resulting dried low rank coal by the combustion heat and exhaust gas from a fluidized bed combustor (FBC) so as to obtain hydrocarbon gas and char. At the same time, electric power is generated by recycling heat with steam from the fluidized bed combustor where the char and the dried low rank coal are present. Furthermore, the reformed char may be used as a fuel for electric power generation and a heat source for steelmaking. On the other hand, the hydrocarbon gas is used as a chemica1 raw material.

Background Art [0002] The low rank coal, such as subbituminous coal or brown coal, which has a moisture content higher than about 20 mass% is limited to use 'within a coal-producing region. This is because, for example, the low rank coal has a low calorie resulting from its high moisture content and generates a small amount of heat by combustion. On the other han.d, when dried, the low rank coal becomes more spontaneously combustible and more hygroscopic, resulting in transportation costs being relatively expensive, etc.

[0003] However, the low rank coal has advantages that are not found, e.g., in the bituminous coal that is considered to be a high rank coal. For example, brown coal found in Australia and Indonesia is low in sulfur content and produces less ash. Thus, using the brown coal as a fuel would make it possible to prevent air pollution due to sulfur dioxide gas, etc., as well as to reduce hazardous ash waste.

[0004] In this context, such techniques have been suggested which are adopted to carbonize the low rank coal by dehydration reform or thermal reform, thereby compensating for the drawbacks thereof. For example, disclosed in Patent Literature 1 and Patent Literature 2 is a technique by which oil and low rank coal are mixed into raw material slurry; the resulting slurry is heated and dehydrated in the oil, and then further heated to decompose or detach the carboxyl radical or the hydroxyl radical, etc., in the raw material coal by a decarboxylation reaction or a dehydration reaction, thereby reforming the raw material coal. Also disclosed is a technique by which heavy oil, etc., is penetrated into pores of the low rank coal so as to prevent spontaneous combustion.

On the other hand, disclosed in Patent Literature 3 is a coal gasification complex power generation facility which includes the following: a gasification unit for gasifying low rank coal having a relatively high moisture content; a gas power generation unit for generating electric power using a gas supplied from the gasification unit; a steam power generation unit for generating electric power by the neat of an exhaust gas emitted from the gas power generation unit; and a coal drying unit for drying coal by the exhaust heat emitted from the steam power generation unit and supplying the dried coal to the gasification unit. Disclosed in Patent Literature 4 is a method for manufacturing reformed coal and hydrocarbon oil by pyrolyzing brown coal into reformed coal and tar under an inert gas atmosphere or steam atmosphere and catalytically cracking the tar in a steam atmosphere and in the presence of an iron-based catalyst so as to obtain hydrocarbon oil. Citation List Patent Literature [ 0005] PTL 1: Japanese Published Unexamined Patent Application

No. H07-233384 PTL 2: Japanese Patent No. 2776278 PTL 3: Japanese Published Unexamined Patent Application No. 2009- 133268 PTL 4: Japanese Published Unexamined Patent Application No. 2010- 144094 [ 0005a] The discussion of documents, acts, materials, devices, articles and the like is included in this specification solely for the purpose of providing a context for the present invention. It is not suggested or represented that any or all of these matters formed part of the prior art base or were common general knowledge in the field relevant to the present invention as it existed before the priority date of each claim of this application.

[ 0005b] Where the terms "comprise", "comprises", "comprised" or "comprising" are used in this specification (including the claims) they are to be interpreted as specifying the presence of the stated features, integers, steps or components, but not precluding the presence of one or more other features, integers, steps or components, or group thereof.

Summary of Invention [ 0006] However, the aforementioned conventional techniques had the following problems: (1) For Patent Literatures 1 and 2, the use of oil requires various types of facilities for separating oil and coal in the same container, causing an increase in the size of the system and impairing energy-saving efficiency; (2) The oil or an indirect material is required for the reforming of the coal, thereby causing a significant increase in costs and imposing a high environmental load; (3) The method which employs the oil causes a heat exchange loss of the energy provided for the brown coal, thus leading to a significant energy loss; (4) Furthermore, the oil used as an indirect material is mixed into the dried coal, thus causing a high loss of oil and impairing resource-saving efficiency; (5) For Patent Literature 3, since the low rank coal is dried and then gasified in a gasification furnace so as to be combusted as a heat source in a boiler, it is possible to obtain a high calorie, but effective use would not be made of a useful chemical raw material contained in the low rank coal, thus impairing resource-saving efficiency; (6) Patent Literature 3 is based on the high-temperature gasification of coal, so that the gas component after gasification is predominantly composed of low molecular-weight compounds and thus disadvantageous to subsequent chemical product synthesis; (7) Patent Literature 3 has a significant restriction on the materials that form the facility because the gases are produced at high temperatures; (8) For Patent Literature 4, the brown coal is pyrolyzed at 500°C to 800°C to obtain the reformed coal and the tar, and then the tar is catalytically cracked at 400 °C to 60 0 °C to thereby obtain the reformed coal and a compound. However, in general, when the low rank coal is heated above 500°C, cracks are increased and fine powder is produced, causing unburned coal to increase . Furthermore, since the pyrolysis gas may cause dangers of easily igniting combustible components or explosion of the powdered coal in a high oxygen concentration, there is a lack of safety and operability because it is difficult to control the operations of the system such as the control of oxygen concentration or addition of steam; and (9) For Patent Literature 4, energy-saving efficiency is impaired because cooling is required -when the brown coal is used as the reformed coal or when the powdered coal is combusted m a downstream stage.

[ 0007] The present invention was developed to address the aforementioned conventional issues. It is therefore an aspect of the invention to provide a complex system for utilizing coal for manufacture of char and raw material gas and electric power generation, the complex system being adopted as follows: (1) To utilize the combustion heat of fixed carbon of coal so as to heat the steam for electric power generation as well as to pyrolyze and gasify the low rank coal and manufacture char; (2) To be capable of making the boiler more compact by employing oxygen fluidized-bed combustion; (3) To be capable of reducing the separation energy of carbon dioxide gas, when the carbon dioxide gas is separated and recycled, by employing oxygen combustion because nitrogen gas is considerably reduced and thus carbon dioxide gas is high in concentration; (4) To be capable of constructing a chemical complex which makes effective use of the exhaust heat from the boiler so as to use a pyrolysis gas and a gasified gas (volatile component) as a chemical raw material; (5) To employ a moving bed reactor as the reformer, whereby the temperature of the product gas may be kept reduced and thus fewer restrictions are imposed on materials such as those for gas pipes, thereby providing outstanding maintainability; (6) To be capable of reducing the temperature of product gas since a long pyrolysis reaction time is available, so that troubles due to a tar component (such as adhesion or caulking) may be solved and a large amount of relatively long-chain hydrocarbon components maybe obtained, producing a gas that is advantageous for combustion and chemical synthesis; (7) To charge the fixed carbon with the volatile component removed into an oxygen fluidized bed combustor without cooling the fixed carbon, thus achieving a high ignition quality and an outstanding energy-saving efficiency; and (8) To be capable of combusting oxygen since high-temperature fixed carbon (char) with volatile components removed may be charged into the oxygen fluidized bed combustor from a portion of a low oxygen concentration in a counterflow relative to the combustion exhaust gas, whereby abnormal combustion or sudden combustion immediately after the chargingmay be suppressed even in the combustor of a high oxygen concentration.

[ 0007a] In another aspect, the present invention provides a system for conversion of coal to char and hydrocarbon gas, comprising: a drying unit in communication with an inert gas supply; a reformer in communication with the drying unit, the reformer comprising: a pyrolysis unit having a counterflow moving bed supplied with downward flowing low rank coal from the drying unit and an ascending flow of the exhaust gas from a fluidized bed combustor, a gasification unit in communication with the pyrolysis unit, a char and ash transfer in communication with the fluidized bed combustor, and a gas outlet in communication with a catalyst reforming unit; wherein the fluidized bed combustor comprises: a supply of oxygen and carbon dioxide, an ash outlet, and an exhaust gas outlet in communication with the reformer; and the catalyst reforming unit comprises: a solid reform catalyst, an outlet for reformed hydrocarbon, a carbon dioxide exhaust pipe in communication with the fluidized bed combustor, and a gas inlet in communication with the reformer.

[ 0008] To address the aforementioned conventional issues, a complex system of the present invention for utilizing coal for manufacture of char and rawmaterial gas and electric power generation is arranged as follows. A complex system according to a first aspect of the present invention for utilizing coal for manufacture of char and raw material gas and electric power generation includes the following: a drying unit for drying low rank coal of a high moisture content; a reformer for reforming the low rank coal that has been dried in the drying unit; a fluidized bed combustor for employing, as a fuel, the reformed coal obtained in the reformer; aproducer gas supplypipe for supplying a combustion exhaust gas from the fluidized bed combustor as a pyrolytic and gasifying agent to the reformer; and a catalyst reforming unit for reforming a volatile component and the combustion exhaust gas obtained from the low rank coal reformed in the reformer.

[ 0009] This arrangement may provide the following operations: (1) Since the low rank coal is dried in the drying unit before being supplied to the reformer, even using the low rank coal as a fuel for the fluidized bed combustor may allow for preventing loss of heat energy that maybe causedby vaporization of the contained moisture or removal of heat due to a leak of the steam, etc.; (2) Heat energy may be used with improved efficiency because the exhaust gas emitted from the fluidized bed combustor is employed for drying the low rank coal. On the other hand, when compared with the case where an additional heat generating unit for generating heat is provided for dry the low rank coal, there is no need to supply an additional fuel or energy, thus achieving an outstanding energy-saving efficiency; (3) Since the reformer is heated with the exhaust gas in the fluidized bed combustor and reforms the low rank coal, an outstanding energy-saving efficiency is achieved; (4) The low rank coal has a high volatile component content; however, the volatile component is emittedby the reformer an.d allowed to react with CO, CO2, or H2O of the combustion gas in the gas reform unit m conjunction with a partially gasified gas, thereby allowing for utilizing the low rank coal as a useful chemical raw material; (0) The char produced in a high temperature portion (inlet portion) in the reform unit may be utilized as raw material coal for steelmaking and a solid fuel that may be transported overseas, and as a fluidized bed fuel; (6) Since the temperature of the producer gas (combustion exhaust gas) from the fluidized bed combustor is used for gas reform, an outstanding thermal efficiency and an outstanding energy-saving efficiency are achieved; (7) Employing the moving bed reactor as the reformer achieves a product gas temperature of as low as 150°C or less and prevents the condensation of the tar. Furthermore, the low temperatures will reduce restrictive conditions on the material such as for gas pipes, thus making it possible to reduce the costs for system construction and maintenance. Furthermore, low-speed heating may prevent the raw material coal from being powderized; (8) Since employing the moving bed reactor as the reformer allows a low product gas temperature and an elongated pyrolysis reaction time, troubles resulting from the occurrence of tar components due to adhesion or caulking, etc., caused by the tar components will not occur, and a large amount of relatively long chain hydrocarbon components may be obtained. It is thus possible to produce gases that are advantageous for chemical raw materials; (9) Since the fixed carbon with the volatile component removed in the reformer is charged into the oxygen fluidized bed combustor without cooling, a high ignition quality7 is achieved and no energy7 loss results; (10) In the fluidized bed combustor, heat may be exchanged with efficiency between the exhaust gas of the f luidizedbed combustor passing by7 against the body7 force of the particle bed and the particles; (11) Since the high-temperature fixed carbon (char) with the volatile component removed is charged into the fluidized bed combustor from a portion of a low oxygen coixcentrat. ion, abnormal combustion or sudden combustion immediately7 after the charging may be suppressed, thus allowing oxygen combustion; and (12) Since the exhaust gas has a lower oxygen concentration than air, the low rank coal that may be spontaneously oxidized and readily catch fire may be reformed at higher temperatures.

[0010] Here, (a) the low rank coal may not be limited to one of a specific name, such as subbituminous coal, lignite, or brown coal as long as the moisture content is above about 20 mass%. Furthermore, all coal to be used as a fuel need not be the low rank coal, but some high rank coal of a moisture content of below about 20 mass% may also be added. (b) The drying unit is dried in the atmosphere of an inert gas such as a nitrogen gas at a low temperature (60°C to 90°C) and a low humidity (RH 70% to 0%) . The inside of the drying unit is made up of a hot water (about 60°C to 90°C) pipe for warming the coal and a gas pipe for injecting a drying inert gas . Furthermore, the target moisture content of the low rank coal may be made 20 mass% or less. In the experiments, the moisture content was reduced to 16 mass%. This made the moisture content of the low rank coal one-third or less, thereby significantly improving transportation efficiency. Furthermore, using the char may prevent spontaneous combustion, thus achieving improved safety.

The nitrogen gas used is the one that is separated in an oxygen separator. The nitrogen gas may be heated in an air preheater which is heated with very hot water of the condenser. In this case, since the oxygen concentration is low, it is possible to prevent the low rank coal, which is spontaneously oxidized and readily increases in temperature as well as readily catches fire, from catching fire, and dry the coal at higher temperatures. Furthermore, since the nitrogen gas separated in the oxygen separator has a low relative humidity, the coal may be dried with increased efficiency. Furthermore, since waste heat is utilized without requiring additional heat energy, the system may be made environmentally friendly and outstanding in energy-saving efficiency. (c) It is possible to recycle clean water from the high humidity exhaust gas discharged from the drying unit, thus making effective use of water. (d) The low rank coal is coarsely crushed, as preprocessing before being dried, into controlled grain sizes of 0.1 ]im to 5 mm. Crushing into grain sizes of 0.1 pm to 5 mm may simplify the drying step so as to shorten the time for drying. The low rank coal is heated by heating the drying chamber of the drying unit using a cooling drain water (about 60°C to 90°C) pipe of the steam condenser of the steam turbine which generates electric power with the steam superheated in the fluidized bed combustor. Furthermore, as a heat transfer medium, air of a low oxygen content, CO2, or N2 gas exchanges heat with the heated cooling drain water and is heated (to a temperature of 60°C to 80°C with RH of 0% to 70%) and is then directed into the drying unit to flow counter to the flow of the low rank coal so as to dry the coal. (e) As the reformer, a preferable one may7 employ tne moving bea scheme by which the low rank coal is pyrolyzed and gasiried while the low rank coal is flowing downwardly and the high-temperature exhaust gas from the fluidized bed combustor is flowing upwardly/. The moving bed scheme allows the moving bed to have an elongated reaction time at the moving bed. Furthermore, the counterflow allows for cooling the gas that has been reformed while being heat exchanged with the low7 rank coal. This makes it possible to obtain a chemical raw material that is made up of a pyrolysis gas and gasification gas as well as to obtain high-calorie reformed coal (char + ash) . (f) In the fluidized bed combustor, employed as a fluidized bed material is limestone or dolomite, etc. As a fuel additive, preferably employed is a gas mixture 01 oxygen and carbon dioxide gas for adjusting (diluting) the concentration of oxygen. The fuel used is dried coal of the low rank coal that has been dried in the drying unit or reformed coal of the low rank coal that has been reformed in the reformer or char. (g) The combustion temperature of the fluidized bed combustor is controlled at 800°C to 900 °C. This allows for reducing use of special materials that withstand high temperatures as the furnace material and for preventing troubles such as melting of ash in the fluidized bed. (h) The catalyst reforming unit performs reforming by allowing the volatile component obtained from the low rank coal or a producer gas {combustion exhaust gas) such as CO 2, CO, and H20 to be brought into contact with the catalyst, thereby yielding, such as, an FT synthesis gas, methanol synthesis gas, ammonia synthesis gas, hydrogen gas, or synthesis natural gas.

Furthermore, a produced tar component may be reformed to continually obtain low molecular-weight hydrocarbon, carbon monoxide, and hydrogen.

[0011] The complex system according to a second asoect of the present invention for utilizing coal for manufacture of char and raw material gas and electric power generation is made up of as follows in the first aspect of the invention: a Pyrolysis unit for-allowing an ascending flow of a combustion exhaust gas of th« fluid 1--^0 bed combustor to decompose the low rank coal supplied from fh« dryina unit at a pyrolysis temperature of 300 °C to 600 °C whiie the reformer is moving the low rank coal; and a gasification unit f-v- _L ci _L L» -L Cl J- -L jg decomposing the low rank coal char produced in the dv- t-....; urij_r from fixed carbon into CO and n2 at 600°C to 800°c.

This arrangement provides the following operations in addi1' i on to those of the first aspect: (1) The dried brown coal may be pyrolyzed into the volatile component + char with the exhaust gas supplied from the fluidized bed combustor, and the char may be further gasified; (2) Unconverted char and ash are supplied to the fluidized bed combustor so as to combust the char, whereby a high calorie may be obtained, thus providing an outstanding thermal efficiency; (3) Since the char contains no moisture, it is possible to achieve a nigh combustion efficiency and considerably reduce heat 1 Ο ς s · ^ ο O f (4) Typically, char is difficult to ignite on its own. However, the char is mixed with the dried brown coal so as to produce an ignition volatile component, or preheated to about 800°C to be combusted in a high oxygen concentration, thereby achieving smooth ignition and combustion; (5) The decomposing in the two stages of the pyrolysis unit and the gasification unit enables char for steelmaking, char as a transportable fuel, and hydrocarbon gas as a chemical raw material to be separated and recycled with high accuracy; (6) Employing the moving bed scheme allows for elongating the reaction time, thereby reducing troubles such as adhesion due to tar; (7) It is possible to choose the component of a gas to be extracted by producing a temperature distribution in the reformer or by selecting a point at which the gas is extracted; (8) The moving bed scheme makes it possible to lower the temperature of the product gas, so that the downstream facility for cooling coal gases, etc., may be eliminated or simplified, thereby making the facility compact; (9) The gasification in the carbon dioxide gas atmosphere ensures high safety; (10) Since no nitrogen gas is contained in the produced gas, the coal gas may be separated with ease; (11) Unlike the fluidized bed in which the temperature in the bed. is uniformed, so that the gasification temperature and the temperature of the pyrolysis gas have to be egual to the temperat'.are in the bed, the moving bed makes it possible to bring the combust-Lon exhaust gas at about 800°C into contact with char at the starting part of the moving bed so as to advance the gasification. In addition, heat absorption and a drop in gas temperature allow for pyrolysis at 300 °C to 600 °C in the middle part of the moving bed while preventing overheating; and (12) The moving bed may be regulated to temperatures or 100°C to 300°C at the uppermost portion depending on the particle bed height. Lowering the temperature of the uppermost portion allows the heavy oil having a relatively high boiling point to be condensed at the upper portion of the particle bed and prevented rrom being distillated. In addition, the heavy oil may be again pyroiyxed and converted into gas, light oil, and char. To obtain the heavy oil, the temperature of the uppermost portion has to be increased to suppress the condensation of the heavy oil.

[0 012] Here, the travel speed of the moving bed may be adjusted according to the feed rate of the char to the fluidized bed combustor. Unlike the case of the fluidized bed where particles are completely mixed resulting in the size of char particles having a significant distribution, the char discharged from the moving bed has a uniform size and thus the fluidized bed combustion may be stabilized with ease. The reformer has a two-stage or an integrated structure, in which the combustion exhaust gas of the fluidized bed combustor is supplied at 500°C to 800°C from the lower portion.

[0013] The complex system according to a third aspect of the present invention for utilizing coal for manufacture of char and raw material gas and electric power generation is adopted m the first or second aspect of the invention such that carbon dioxide gas supplied as a diluent for fuel additive oxygen to the fluidized bed combustor is a carbon dioxide gas discharged and separated from the catalyst reforming unit.

This provides the following operation in addition to those of the first or second aspect: (1) The carbon dioxide gas discharged from the fluidized bed combustor and the reformer is recycled, thus providing an improved effect of reducing environmental loads.

Advantageous Effects of Invention [0014] As described above, the complex system of the present invention for utilizing coal for manufacture of char and raw material gas and electric power generation provides the following adv a nt age o u s effects.

The first aspect of the invention provides the following advantageous effects: (1) Since the low rank coal is dried in the drying unit before being supplied to the reformer, it is possible to suppress the vaporization of the moisture contained in the low rank coal of a high moisture content and the loss of heat energy due to removal of heat by the leakage of steam, etc.; (2) Since the low rank coal is dried using the exhaust heat emitted from the fluidized bed combustor or the waste neat produced in the power generation cycle, it is possible to utilize heat energy with improved efficiency. On the other hand, when compared with the case where there is provided an additional heat generating unit for generating heat so as to dry the low rank coal, no additional fuel or energy needs to be charged and thus an outstanding energy-saving efficiency is achieved; (3) The reformer is heated by the exhaust gas from the fluidized bed combustor for reform and gasification, thus achieving an outstanding thermal efficiency; (4) The low rank coal has a high volatile component content; however, the volatile component and the gasified gas react with CO, C02, or H20 of the combustion gas in the gas reform unit, thereby allowing for converting and utilizing the coal as a useful chemical raw material; (5) Since the temperature of the exhaust gas from the fluidized bed combustor is used for gas reform, an outstanding thermal efficiency and an outstanding energy-saving efficiency' are achieved; ( 6) The temperature of the product gas to be produced is reduced by employing the moving bed reactor as a pyrolysis and gasification unit, thereby reducing restrictive conditions on the materials such as for gas pipes; (7) At the same time, the pyrolysis reaction time may be elongated by employing the moving bed. Thus, this prevents troubles due to tar components (such as adhesion or caulking) and makes it possible to obtain a large amount of relatively long-chain hydrocarbon components, allowing for producing a gas advantageous for chemical product synthesis; (8) Since the fixed carbon with the volatile component removed is charged into the oxygen fluidized bed combustor without cooling, a nigh ignition quality is achieved and no energy' loss results; and (9) Since the nigh-temperature fixed carbon (char) with the volatile component removed is supplied to the oxygen fluidized bed combustor in a counterflow direction relative to the exhaust gas and thus may be charged into the oxygen fluidized bed combustor from a portion of a low oxygen concentration, abnormal combustion or sudden combustion immediately after the charging maybe suppressed, thus allowing oxygen combustion.

[0015] The second aspect of the invention provides the following advantageous effects in addition to those of the first aspect: (1) The dried brown coal is py roly zed into volatile components and char with the combustion gas supplied from the fluidized bed combustor, and the char is further gasified; (2) Unconverted char and ash are supplied to the fluidized bed combustor so as to combust the char, whereby a high calorie may be obtained, thus providing a high thermal efficiency; (3) Since the char contains no moisture, a high combustion efficiency and no heat loss are achieved; (4) Typically, char is difficult to ignite on its own. However, the char is preheated to about 800 °C to be combusted in a high oxygen concentration, thereby achieving smooth ignition and combustion; (5) Employing the moving bed scheme allows for elongating the reaction time, thereby reducing troubles such as adhesion due to tar; (6) It is possible, by producing a temperature distribution, to choose the component of a gas at a point at which the gas is extracted; and (7) The moving bed scheme for the pyrolysis and gasification unit makes it possible to lower the temperature of the product gas, so that the downstream facility for cooling coal gases, etc., may be eliminated, thereby providing an outstanding energy-saving efficiency and making the facility compact.

[0016] The third aspect of the invention provides the following advantageous efrects rn addition to those of the first or second aspect: (1) The carbon dioxide gas discharged from the fluidized bed combustor and the reformer is recycled, thus providing an improved effect of reducing environmental loads; (2) Use of an inert gas for drying, thereby reducing the danger of explosion, etc.; and (3) Since CO2 has a high specific heat, heat may be transferred with ease (i.e., the cooling efficiency is high).

Brief Description of Drawings [0017] Fig. 1 is a schematic view illustrating a complex system according to an embodiment for utilizing coal for manufacture of char and raw material etas and electric power generation.

Fig. 2 is a view of heat balance according to an embodiment. Fig. 3 is a view of material balance according to an embodiment. Description of Embodiments [0018] Hereinafter, description will be made to the mode for-carrying out the present invention with reference to the drawings.

Fig. 1 is a schematic view illustrating a complex system according to an embodiment for utilizing coal for manufacture of char and raw material gas and electric power generation.

Fig. 1 shows a complex system 1 for utilizing coal for manufacture of char and raw material gas and electric power generation. The complex system 1 includes a drying unit 2 for drying low rank coal such as brown coal, which is in the shape of lump coal having a grain size of 1 μια to 5 mm and a moisture content of generally 60 mass%, using the gas flow or an inert gas sucn as air having a low oxyaen content or nitrogen of which temperature and relative humidity are controlled at 60°C to 80°C and 0% to /0%, respectively. The drying is continued until the moisture content becomes 20 mass%. In this implementation example, the drying chamber of the drying unit 2 includes a pipe for 60°C to 90°C hot water connected to a condenser (to be discussed later) for warming the coal, and a gas pipe for injecting an N2 gas into the drying chamber, the N2 gas being separated in an oxygon separator (to be discussed later) and heated in an air preheater (to be discussed later). The moisture in the exhaust gas in the drying unit 2 is recycled by makeup water treatment and supplied to the condenser. The complex system 1 also includes a dust collector 2a for removing dust particles, etc., from the exhaust gas of the drying unit 2. Further included is a reformer 3 that is adopted to reform the low rank coal, which has been dried in the drying unit 2 and transferred in a transfer material, in two-stage reactions of pyrolysis and partial gasification, and vaporize and detach volatile components and tar components, etc., so as to reform the low rank coal into char, ash, and coal gas. The reformer 3 is capable of performing the reform in the two-stage reactions of the pyrolysis and partial gasification, thereby' adapting the physical properties of the product char to the requirements for service. Also included are the following: a fluidized bed combustor 4 to which the char and ash reformed in the reformer 3 (hereafter ref erred to as the reformed coal) is supplied so as to produce main steam for a steam turbine; a cyclone 5 for removing ash from the exhaust gas of the fluidized bed combustor 4; an oxygen preheater 6 for exchanging heat between the exhaust gas separated in the cyclone 5 and the oxygen separated in an oxyaen separator (to be discussed later) so as to preheat the oxygen gas; and an oxygen separator 7 for separating the oxygen gas and the nitrogen gas from the atmosphere. The oxygen gas obtained from the oxygen separator 7 is preheated in the oxygen preheater 6 and used as a fuel additive for the fluidized bed combustor 4. Furthermore, the nitrogen gas obtained at the same time is heated and used to dry the low rank coal. Further included are the following: a cyclone 8 for separating ash, etc . , from a gasified gas that includes volatile compοnents or tar compοnents gasif ied with a gasif ying agent composed of the exhaust gas from the fluidized bed combustor when the low rank coal is reformed in the reformer 3; a catalyst reforming unit 9 which brings the gasif ied gas with the ash separated in the cyclone 8 into contact with a catalyst such as zeolite, Fe, Co, Ni, or Cu so as to refine a chemical raw material such as an FT synthesis gas, methanol synthesis gas, ammonia synthesis gas, hydrogen gas, or synthesis natural gas; a carbon dioxide gas pipe rO for supplying, as a CCS, the combustion exhaust gas or the carbon dioxide gas produced (as a by-product) in the catalyst reforming unit 9 as a diluent for the concentration of the oxygen gas in a carbon dioxide gas reservoir unit and the fluidized bed combustor 4; a steam turbine 11 for rotating a power generator with the main steam of the fluidized bed combustor 4; a condenser i2; a power generator 13; and a drying aas preheater 14 for allowing the very hot water of the condenser 12 to heat the nitrogen gas separated in the oxygen separator 7. The nitrogen gas preheated in the drying gas preheater 14 is fed into the drying unit 2 so as to dehydrate and dry the low rank coal. Also included are the following: a water feedpump 15 for pressurizing feedwater to supply condensate from the condenser 12 into a combustor heat transfer water pipe; a feedwater heater 16 for allowing the steam (extracted vapor) from the turbine to preheat the condensate from the water feed pump 15; and a cooling tower 17, Γ0019] The complex system, arranged as described above, for utilizing coal for manufacture of char and raw material gas and electric power generation will be described as follows in terms of each unit operation. (1) The low rank coal is coarsely crushed in advance, e.g., in a ball mill and separated and transferred in an air current, and then supplied to the drying unit 2 of the complex system for utilizing coal for manufacture of char and raw material gas and e 1 e c t r i c p o w e r g e n e r a t i ο n . (2) In the drying unit 2, a drying gas of a relative humidity of 0% to 70% at a temperature of 65°C to 110°C is employed so that the moisture content of the low rank coal with the grain size controlled to 0.1 pm to 5 mm is lowered to 20 mass% or less. The drying gas to be employed is the waste heat that is recycled from the steam turbine, the combustor fluidized bed material, and the reformed coal product. (3) The reformer 3 preferably employs the moving bed scheme by taking slagging measures into account, in the case of which the combustion exhaust gas with the high-temperature portion controlled serves as a pyrolytic andpartial gasifying reform agent. This allows for elongating the reaction time and preventing troubles such as caulking of tar components . Furthermore, the cracking of a component having a long carbon chain may be accelerated and as well allowed to serve to cool a product coal gas, thereby facilitating the handling of the produced coal gas.

The reformer may take advantage of a two-stage rotary kiln. This allows for selecting between direct heating/ref orm and indirect heating by the combustion gas. The reformed coal may be set by the combustion gas to 600°C to 500°C and an inlet dried coal charge t emp e ra t ure o f 3 0 0 0 C t o 4 0 0 0 C. (4) The fluidized bed combustor 4 employs a fuel additive that is obtained by allowing the oxygen separated in the oxygen separator 7, which separates oxygen from atmosphere, to be diluted with the carbon dioxide gas produced {as a by-product) or separated from the catalyst reforming unit 9. (5) The catalyst reforming unit 9 employs a solid reform catalyst such as iron or an alkaline component. More specifically, it is possible to utilize a f ixedbed, etc . , which employs a perovskite carrying alkaline earth catalyst. This makes it possible to decompose a heavy component such as a tar component into a light component.

[0020] The low rank coal to be employed may be subbiturn!nous coal, low moisture content brown coal (lignite), or high moisture content brown coal (brown coal) . The moisture content and neat value thereof are shown in (Table 1).

[0021] [Table 1]

[0022] The low rank coal moisture is divided into surface adhesion moisture and internal moisture {equilibrium moisture), where the surface adhesion moisture may be dried and removed at 100°C or less.

The moisture of coal may be reduced to about one-half of the equilibrium moisture by being dried at 80 °C to 150 °C (also referred to as typical drying) . However, heating and drying at 150 °C or less ~eauce the tendency to reform the low rank coal. In this context, the arying unit 2 employed an N2 gas at a temperature of 60°C to 10 c 'with a relative humidity of 0% to 70%.

Next, heating at about 180 °C to 300 °C would cause a hydrophilic x-?gen containing group such as the phenol group or the carboxyl ^ °UP to have a tendency to be pyiolyzed. The internal moisture ^ t" o ~ °oal is removed by heating, and the hydrophilic oxygen c°ntajr .. nirig group such as the phenol group and the carboxyl group J-S Qj ^ '°mPosed to produce H20 and C02 and turned to be hydrophobic, r®suit ; n ^9 in degradation in the hygroscopicity of the coal. Furthev· * '“note, the oxygen content in the coal is reduced and thereby -‘-hact iv-N + ated, thus suppressing spontaneous combustion to some extent. * atthermore, heating to 300 °C or higher causes the equilibrium mo a. ,,+. to start to reduce and considerably reduce at 350°C or one-half or less of the equilibrium moisture by the typical this time, the tar component in the coal is liquefied enu,,, to the surface throuqh the pores of the coal. From the $5 r-i " ^hriij- electron micrograph of the surface and by the measurement °f the ,,. ., specific surface area, this mav also be seen from the fact 'hat the ' coal specific surface area is considerably reduced. For example, when raw material coal of a specific surface area of 1.7 ϊτΓ/g is heated at 4 30°C and then rapidly cooled, the specific surface area is reduced to about 0.1 rrk/g.

Tne tar component which is spread inside the pores and over pa.rt oi che coal surface and solidified is considered to cause the coal to be reduced in specific surface area and inactivated so as to be degraded in hygroscopicity as well as in spontaneous combustion property . Furthermore, heating over 4 50 °C to about 50 0°C would cause the equilibrium moisture to be further reduced; however, from the scanning electron micrograph and the measurement of the specific surface area, a number of cracks are found on the surface of the coal and the specific surface area sharply increases to about 2.4 m2/g .

Furthermore, when heating over 50 0 °C, the coal tends to have more cracks and become brittle, causing generation of fine powder to increase. In this context, the reformer 3 employing the moving bed makes it possible to prevent the coal from being powderized due to the low-speed heating with the moving bed.

[0023] On the other hand, the high moisture content brown coal of a moisture content of 65 mass% has an amount of moisture of about 1x65/(100-65) that is approximately equal to 1.86 kg per 1 kg of dried coal. Thus, since the brown coal of a high moisture content has a moisture loss of 1.8 6 kg from a chimney and the moisture loss is 650 kcal per 1 kg of water, the moisture loss is 650xi ♦ 86=120^ kcal per 1 kg of dried coal. Therefore, the heat quantity that may be converted to steam is 5720-1209 = 4511 kcal per 1 kg of dried coal. The effectively employable heat quantity ratio of the high moisture content brown coal to the bituminous coal (the heat quantity that may be converted into steam is 5720 kcal) is 4511/5720 that is approximately equal to 7y%.

[0024] According to Table 1, the high moisture content brown coal provides a power generation efficiency of 28%, and when compared with 34.5% of the bituminous coal (moisture content: 5 mass%), it holds that 28.0/34.5 approximately equal to 81%, which is generally equal to the aforementioned heat quantity ratio. That is, the heat quantity ratio between the two types of coal is equal to the difference between the moisture losses. In this context, to increase the heat quantity of the low rank coal by dehydration reform in order to generate electric power with the low rank coal employed as a fuel, the heat quantity had to be increased by the moisture loss or more, that is, the steam consumption required for treating I kg of water was a consumption of 1 kg steam or more according to the conventional dehydration reform method.

[0025] In this context, the inventors have intensively made a close study of the complex system for utilizing coal, which is high in calorie and power generation efficiency, for manufacture of char and raw material gas and electric power generation and completed as an invention, the complex system being adopted to vaporize the moisture of the low rank coal with a small amount of heat energy as well as to detach the high volatile component with the energy of the combustion gas so as to utilize the same not as a fuel but as a raw material for chemical products.

[0026] Furthermore, an operation method of the system includes the following steps: a grain size control step of controllably crushing low rank coal into grain sizes of about 0.1 pm to 5 mm; a drying step of drying the low rank coal having controlled grain sizes to a moisture content of 20 mass% or less; a reforming step of using an exhaust gas from a fluidized bed combustor to reform the dried coal dried in the drying step; a catalyst reiorm step of reforming the gasified gas reformed in the reiorm step no a chemical raw material; a combustion step of combusting, in the fluidized bed combustor, the reformed coal (char and ash) reformed in the reform step so as to produce steam; and a power generation step of generating electric power by the steam. Eurthermore, the operation method is achieved by the reform step including a pyroiysis s t e p f o r ρ y r o 1 y z i n g the dried c o a 1 andagasxricati ο n s L e ρ of g a s i f y r n a the pyrolysed and dried coal. The char that may be excessively produced may be employed as a steelmaking raw carbon maierial ana a transportable solid fuel.

[0027] Next, a computer simulation was performed on tne heat balance and the material balance of the complex system according to this embodiment for utilizing coal for manufacture of char ana raw material gas and electric power generation. As a conaition, unworked brown coal of Victorian origin was employed as low rariK coal. The initial moisture of the brown coal was 6U mass%, the moisture of dried brown coal 'when dried in the drying unit 2 was 20 mass%, the fuel ratio was 1.2, and electric power was generated with an efficiency of 30%.

The results are shown in Figs. 2 and 3.

Fig. 2 is a view showing si neat balance according to the embodiment, and Fig. 3 is a view showing a material balance according to the embodiment.

From Figs. 2 and 3, when the moisture of the fuel brown coal is reduced, the heat energy that may be utilized for electric power generation is increased, that is, the amount of power generation is increased. It is also seen that the exhaust heat that is proaucea in the power generation process is used for the drying energy, ΐ. hereby providing increasedefficiency. Furthermore, reducing the moisture of the brown coal may cause an increase in the produced retort gas enthalpy, th US cl C il ieving a further improved efficiency in the retorting operation. Furthermore, employing CO2 circulation facilitates the recycle of CO2 even when CO2 storage is targeted. Industrial Applicability [0028] According to the present invention, dried low rank coal is pyroiysed and gasified, while being moved in a reformer such as the moving bed, by the combustion heat of reformed brown coal m the fluidized bed combustor (FBC) so as to recycle hydrocarbon gas and char, etc., and the reformed char is supplied to the oxygen fluidized bed combustor so as to produce steam for electric power generation, thereby generating electric power and producing C02 gas at a controlled supply temperature for pyrolysis and gasification. This allows for providing a complex system which is capable of utilizing coal for manufacture of char and raw material gas and electric power generation by merging electric power generation and coal chemistry so as to make full use of heat, electricity, and chemical products.

Reference Signs List [0029] 1: complex system for utilizing coal in manufacture of char and raw material gas and electric power generation 2: drying unit 3: reformer 4: fluidized bed combustor 5: cyclone 6: oxygen preheater 7: oxygen separator 8: cyclone 9: catalyst reforming unit 10: carbon dioxide gas pipe 11: steam turbine 12: condenser 13: power generator 14: drying gas preheater 15: water feed pump 16: feedwater heater 17: cooling tower

Claims

THE CLAIMS DEFINING THE INVENTION ARE AS FOLLOWS:

1. A system for conversion of coal to char and hydrocarbon gas, comprising: a drying unit in communication with an inert gas supply; a reformer in communication with the drying unit, the reformer comprising: a pyrolysis unit having a counterflow moving bed supplied with downward flowing low rank coal from the drying unit and an ascending flow of the exhaust gas from a fluidized bed combustor, a gasification unit in communication with the pyrolysis unit, a char and ash transfer in communication with the fluidized bed combustor, and a gas outlet in communication with a catalyst reforming unit; wherein the fluidized bed combustor comprises: a supply of oxygen and carbon dioxide, an ash outlet, and an exhaust gas outlet in communication with the reformer; and the catalyst reforming unit comprises: a solid reform catalyst, an outlet for reformed hydrocarbon, a carbon dioxide exhaust pipe in communication with the fluidized bed combustor, and a gas inlet in communication with the reformer.
2 . The system for conversion of coal according to claim 1, wherein a temperature of the pyrolysis unit is from 150°C to 600°C; and a temperature of the gasification unit is from 600°C to 800°C.
3. The system for conversion of coal according to claim 1 or 2, further comprising an oxygen separator which supplies oxygen to the fluidized bed combustor and nitrogen as an inert gas to the drying unit.
4 . The system for conversion of coal according to any one of claims 1 to 3, wherein the fluidized bed combustor comprises limestone or dolomite as a fluidized bed material and a temperature of the fluidized bed combustor is from 800°C to 900°C.
5 . A method for conversion of low rank coal to char and hydrocarbon gas employing the system for conversion of coal of any one of claims 1 to 4, comprising: crushing the low rank coal to a grain size of 0.1 pm to 5 mm; drying the crushed low rank coal to a maximum moisture content of 20% by mass or less under flow of an inert gas at a temperature of from 60°C to 90°C in the drying unit to obtain a crushed coal; transferring the crushed coal to the reformer; pyrolyzing and contacting the crushed coal with an exhaust gas from the fluidized bed combustor in the reformer to obtain a combined pyrolysis and gasification gas and a reformed coal comprising char and ash; transferring the reformed coal to the fluidized bed combustor; transferring the combined pyrolysis and gasification gas to the catalyst reforming unit; combusting the char in the fluidized bed combustor with a supply of oxygen diluted with carbon dioxide at a temperature of from 800°C to 900°C; and reforming the combined pyrolysis and gasification gas in the catalyst reforming unit to obtain the hydrocarbon gas.